Growth of structural lengthscale in Kob–Andersen binary mixtures: Role of medium range order

A central and extensively debated question in glass physics concerns whether a single, growing lengthscale fundamentally controls glassy dynamics, particularly in systems lacking obvious structural motifs such as the Kob-Andersen binary Lennard-Jones (KALJ) model. In this work, we investigate structural and dynamical lengthscales in supercooled liquids using the KALJ model in two compositions: 80:20 and 60:40. We compute the dynamical lengthscale from displacement-displacement correlation functions and observe a consistent growth as temperature decreases. To explore the static counterpart, we use a structural order parameter (SOP) based on the mean field caging potential. While this SOP is known to predict short time dynamics effectively, its bare correlation function reveals minimal spatial growth. Motivated by recent findings that long time dynamics reflect collective rearrangements, we perform spatial coarse-graining of the SOP and identify an optimal lengthscale Lmax that maximizes structure-dynamics correlation. We show that the structural correlation length derived from SOP coarse-grained over Lmax exhibits clear growth with cooling and closely tracks the dynamical lengthscale, especially for A particles in the 80:20 mixture and for both A and B particles in the 60:40 system. Our results reconcile the previously observed absence of static length growth in the KALJ model by highlighting the necessity of intermediate range structural descriptors. Furthermore, we find that the particles with larger structural length growth also correspond to species with latent crystallization tendencies, suggesting a possible link between structural order, dynamics, and incipient crystallization.

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Journal
The Journal of Chemical Physics
Published
2025-11-25
DOI
https://doi.org/10.1063/5.0292633
Primary Topic
Material Dynamics and Properties
Type
article
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article

Growth of structural lengthscale in Kob–Andersen binary mixtures: Role of medium range order

Indrajit Tah, Sarika Maitra Bhattacharyya, Mohit Sharma, Sanket Kumawat et al.
The Journal of Chemical Physics
Material Dynamics and Properties
article

Growth of structural lengthscale in Kob–Andersen binary mixtures: Role of medium range order

Indrajit Tah, Sarika Maitra Bhattacharyya, Mohit Sharma, Sanket Kumawat, Ujjwal Kumar Nandi
article en

Abstract

A central and extensively debated question in glass physics concerns whether a single, growing lengthscale fundamentally controls glassy dynamics, particularly in systems lacking obvious structural motifs such as the Kob-Andersen binary Lennard-Jones (KALJ) model. In this work, we investigate structural and dynamical lengthscales in supercooled liquids using the KALJ model in two compositions: 80:20 and 60:40. We compute the dynamical lengthscale from displacement-displacement correlation functions and observe a consistent growth as temperature decreases. To explore the static counterpart, we use a structural order parameter (SOP) based on the mean field caging potential. While this SOP is known to predict short time dynamics effectively, its bare correlation function reveals minimal spatial growth. Motivated by recent findings that long time dynamics reflect collective rearrangements, we perform spatial coarse-graining of the SOP and identify an optimal lengthscale Lmax that maximizes structure-dynamics correlation. We show that the structural correlation length derived from SOP coarse-grained over Lmax exhibits clear growth with cooling and closely tracks the dynamical lengthscale, especially for A particles in the 80:20 mixture and for both A and B particles in the 60:40 system. Our results reconcile the previously observed absence of static length growth in the KALJ model by highlighting the necessity of intermediate range structural descriptors. Furthermore, we find that the particles with larger structural length growth also correspond to species with latent crystallization tendencies, suggesting a possible link between structural order, dynamics, and incipient crystallization.

The Journal of Chemical PhysicsVol. 163(20)
Central Glass and Ceramic Research Institute (IN), Kyoto University (JP), National Chemical Laboratory (IN), Institute of Polymers (BG), Kyoto University of Education (JP), Academy of Scientific and Innovative Research (IN)
Openalex Percentile: Top 70%
Material Dynamics and Properties
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